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The importance of organic aerosol particles in the environment has been long established, influencing cloud formation and lifetime, absorbing and scattering sunlight, affecting atmospheric composition and impacting on human health. Conventionally, ambient organic particles were considered to exist as liquids. Recent observations in field measurements and studies in the laboratory suggest that they may instead exist as highly viscous semi-solids or amorphous glassy solids under certain conditions, with important implications for atmospheric chemistry, climate and air quality. This review explores our understanding of aerosol particle phase, particularly as identified by measurements of the viscosity of organic particles, and the atmospheric implications of phase state. The phase state of organic particles in the atmosphere has important consequences for the impact of aerosols on climate, visibility, air quality and health. Here, the authors review the evidence for the formation of amorphous glassy particles and the methods for determining aerosol particle viscosity.

We examine the hygroscopic properties of particles freshly emitted from laboratory biomass burning experiments conducted during the second Fire Lab At Missoula Experiment (FLAME‐II). Values of the hygroscopicity parameter, kappa, were derived from both hygroscopic growth measurements and size‐resolved (30–300 nm in diameter) cloud condensation nuclei (CCN) measurements for smokes emitted by the open combustion of 24 biomass fuels from the United States and Asia. To analyze the complex cloud condensation nuclei response curves we propose a new inversion scheme that corrects for multiple charge effects without the necessity of prior assumptions about the chemical composition and mixing state of the particles. Kappa varied between 0.02 (weakly hygroscopic) and 0.8 (highly hygroscopic). For individual smokes, kappa was a function of particle size, with 250 nm particles being generally weakly hygroscopic and sub‐100 nm particles being more hygroscopic. At any given size the emissions were often externally mixed, showing more and less hygroscopic growth modes and bimodal CCN activation spectra. Comparisons between growth factor‐derived and CCN‐derived hygroscopicities were consistent when taking this heterogeneity into account. A conceptual model of biomass burning emissions suggests that most particles are CCN active at the point of emission and do not require conversion in the atmosphere to more hygroscopic compositions before they can participate in cloud formation and undergo wet deposition.

Cloud water sedimentation and drizzle in a stratocumulus-topped boundary layer are the focus of an intercomparison of large-eddy simulations. The context is an idealized case study of nocturnal stratocumulus under a dry inversion, with embedded pockets of heavily drizzling open cellular convection. Results from 11 groups are used. Two models resolve the size distributions of cloud particles, and the others parameterize cloud water sedimentation and drizzle. For the ensemble of simulations with drizzle and cloud water sedimentation, the mean liquid water path (LWP) is remarkably steady and consistent with the measurements, the mean entrainment rate is at the low end of the measured range, and the ensemble-average maximum vertical wind variance is roughly half that measured. On average, precipitation at the surface and at cloud base is smaller, and the rate of precipitation evaporation greater, than measured. Including drizzle in the simulations reduces convective intensity, increases boundary layer stratification, and decreases LWP for nearly all models. Including cloud water sedimentation substantially decreases entrainment, decreases convective intensity, and increases LWP for most models. In nearly all cases, LWP responds more strongly to cloud water sedimentation than to drizzle. The omission of cloud water sedimentation in simulations is strongly discouraged, regardless of whether or not precipitation is present below cloud base.

During the CalWater 2015 field campaign, ground-level observations of aerosol size, concentration, chemical composition, and cloud activity were made at Bodega Bay, CA, on the remote California coast. A strong anthropogenic influence on air quality, aerosol physicochemical properties, and cloud activity was observed at Bodega Bay during periods with special weather conditions, known as Petaluma Gap flow, in which air from California's interior is transported to the coast. This study applies a diverse set of chemical, cloud microphysical, and meteorological measurements to the Petaluma Gap flow phenomenon for the first time. It is demonstrated that the sudden and often dramatic change in aerosol properties is strongly related to regional meteorology and anthropogenically influenced chemical processes in California's Central Valley. In addition, it is demonstrated that the change in air mass properties from those typical of a remote marine environment to properties of a continental regime has the potential to impact atmospheric radiative balance and cloud formation in ways that must be accounted for in regional climate simulations.

Biomass burning is a significant source of carbonaceous aerosol in many regions of the world. When present, biomass burning particles may affect the microphysical properties of clouds through their ability to function as cloud condensation nuclei or ice nuclei. We report on measurements of the ice nucleation ability of biomass burning particles performed on laboratory‐generated aerosols at the second Fire Lab at Missoula Experiment. During the experiment we generated smoke through controlled burns of 21 biomass fuels from the United States and Asia. Using a Colorado State University continuous flow diffusion chamber, we measured the condensation/immersion freezing potential at temperatures relevant to cold cumulus clouds (−30°C). Smokes from 9 of the 21 fuels acted as ice nuclei at fractions of 1:10,000 to 1:100 particles in at least one burn of each fuel; emissions from the remaining fuels were below the ice nuclei detection limit for all burns of each fuel. Using a bottom‐up emission model, we estimate that smokes that emit ice nuclei fractions exceeding 1:10,000 particles can perturb ice nuclei concentrations on a regional scale.

Aerosol hygroscopicity is a critical parameter for predicting radiative forcing and climate sensitivity, particularly under sub-saturated regimes where it drives complex aerosol–water interactions. Here, we show that externally mixed aerosols exert a stronger influence on direct radiative forcing than is currently represented in models. Incorporating our findings into radiative forcing calculations indicates a stronger aerosol cooling effect, especially at suburban sites, highlighting the importance of representing regional differences in mixing state. The conventional bulk-chemistry approach, which assumes volume-based mixing with limited spatial variability, exhibits low predictive performance for aerosol hygroscopicity (R² ≈ 0.61) at urban and suburban sites. Using an interpretable machine learning framework trained on geographically diverse, region-specific datasets can capture this variability with higher accuracy (R² ≈ 0.97), identifying key chemical compositional and mixing-state drivers. Incorporating regional diversity of aerosol hygroscopicity provides a more accurate representation of aerosol hygroscopicity in climate models, according to a machine learning approach trained on aerosol observational data.

Tikhonov regularization is a tool for reducing noise amplification during data inversion. This work introduces RegularizationTools.jl, a general-purpose software package for applying Tikhonov regularization to data. The package implements well-established numerical algorithms and is suitable for systems of up to ∼ 1000 equations. Included is an abstraction to systematically categorize specific inversion configurations and their associated hyperparameters. A generic interface translates arbitrary linear forward models defined by a computer function into the corresponding design matrix. This obviates the need to explicitly write out and discretize the Fredholm integral equation, thus facilitating fast prototyping of new regularization schemes associated with measurement techniques. Example applications include the inversion involving data from scanning mobility particle sizers (SMPSs) and humidified tandem differential mobility analyzers (HTDMAs). Inversion of SMPS size distributions reported in this work builds upon the freely available software DifferentialMobilityAnalyzers.jl. The speed of inversion is improved by a factor of ∼ 200, now requiring between 2 and 5 ms per SMPS scan when using 120 size bins. Previously reported occasional failure to converge to a valid solution is reduced by switching from the L-curve method to generalized cross-validation as the metric to search for the optimal regularization parameter. Higher-order inversions resulting in smooth, denoised reconstructions of size distributions are now included in DifferentialMobilityAnalyzers.jl. This work also demonstrates that an SMPS-style matrix-based inversion can be applied to find the growth factor frequency distribution from raw HTDMA data while also accounting for multiply charged particles. The outcome of the aerosol-related inversion methods is showcased by inverting multi-week SMPS and HTDMA datasets from ground-based observations, including SMPS data obtained at Bodega Marine Laboratory during the CalWater 2/ACAPEX campaign and co-located SMPS and HTDMA data collected at the US Department of Energy observatory located at the Southern Great Plains site in Oklahoma, USA. Results show that the proposed approaches are suitable for unsupervised, nonparametric inversion of large-scale datasets as well as inversion in real time during data acquisition on low-cost reduced-instruction-set architectures used in single-board computers. The included software implementation of Tikhonov regularization is freely available, general, and domain-independent and thus can be applied to many other inverse problems arising in atmospheric measurement techniques and beyond.

The vertical distribution of freshly nucleated aerosol particles in the marine boundary layer remains poorly constrained, limiting our ability to represent new particle formation in climate models. Here we characterize 3–10 nm particle events, termed small particle events (SPEs), by deriving their vertical turbulent fluxes from aircraft measurements during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. To overcome stationarity limitations of traditional eddy covariance methods, we applied continuous wavelet transform analysis to data collected during June–July 2017 and January–February 2018 flights over the Azores. Our flux-based analysis revealed two distinct SPE scenarios with different vertical structures and spatial extents. The first featured nucleation in the entrainment zone, where free tropospheric air entrains into the boundary layer. The second showed nucleation in the decoupled layer, a stratified region between the well-mixed surface layer and cloud-topped upper boundary layer. In both cases, convergence of air masses from different layers diluted preexisting aerosol surface area to very low levels, creating conditions favorable for nucleation and generating strong downward particle fluxes. SPEs occurred in 15 % of flights, challenging prevailing theoretical expectations that new particle formation should rarely occur in marine boundary layers due to high condensation and coagulation sink capacity of sea spray aerosols. Aircraft-derived particle fluxes provide first observational constraints on the vertical location and source strength of likely nucleation regions in the remote marine boundary layer, improving aerosol source representations in climate models and reducing uncertainties in aerosol-cloud interactions.

Measurements of ice formation by biomass combustion particles generated in controlled laboratory burns were made using a continuous flow diffusion chamber operating in the temperature range between −45 and −60°C. These measurements are the first of their kind to investigate the role that such particles may play in ice formation in upper tropospheric clouds. Measurements of aerosol water uptake were used to examine the role of hygroscopicity in low‐temperature ice nucleation by biomass combustion particles. Ice formation by the smoke particles at below −45°C and below water saturation followed the temperature and relative humidity dependencies predicted for water activity‐based homogeneous freezing within measurement uncertainties. As predicted, relative humidity dependence of homogeneous freezing fractions on hygroscopicity was weak in comparison with the temperature dependence for biomass particles of typical atmospheric sizes. The action of heterogeneous ice nucleation in or on these small smoke particles in the haze particle regime could not be distinguished within measurement uncertainties. Impedance of homogeneous freezing below −50°C was inferred for freezing higher number fractions of predominantly organic smoke particles separately reported to contain an abundance of large organic molecules, consistent with the recently predicted onset conditions for and impact of viscous or glassy aerosol phase states. Finally, we note that precision and accuracy requirements of instrumentation for resolving modest impacts (a few degrees less supercooling or a few percent lower relative humidity) of heterogeneous freezing, as compared with homogeneous freezing in the upper tropospheric temperature regime present difficulties for validating aerosol impacts on cirrus.

Atmospheric aerosols can exist in amorphous semi-solid or glassy phase states whose viscosity varies with atmospheric temperature and relative humidity. The temperature and humidity dependence of viscosity has been hypothesized to be predictable from the combination of a water–organic binary mixing rule of the glass transition temperature, a glass-transition-temperature-scaled viscosity fragility parameterization, and a water uptake parameterization. This work presents a closure study between predicted and observed viscosity for sucrose and citric acid. Viscosity and glass transition temperature as a function of water content are compiled from literature data and used to constrain the fragility parameterization. New measurements characterizing viscosity of sub-100 nm particles using the dimer relaxation method are presented. These measurements extend the available data of temperature- and humidity-dependent viscosity to −28 ∘C. Predicted relationships agree well with observations at room temperature and with measured isopleths of constant viscosity at ∼107 Pa s at temperatures warmer than −28 ∘C. Discrepancies at colder temperatures are observed for sucrose particles. Simulations with the kinetic multi-layer model of gas–particle interactions suggest that the observed deviations at colder temperature for sucrose can be attributed to kinetic limitations associated with water uptake at the timescales of the dimer relaxation experiments. Using the available information, updated equilibrium phase-state diagrams (-80∘C

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